Measurements of joint kinematics are essential to understand the pathomechanics of ankle disease and the effects of treatment. Traditional motion capture techniques do not provide measurements of independent tibiotalar and subtalar joint motion. In this study, high-speed dual fluoroscopy images of ten asymptomatic adults were acquired during treadmill walking at 0.5 m/s and 1.0 m/s and a single-leg, balanced heel-rise. Three-dimensional (3D) CT models of each bone and dual fluoroscopy images were used to quantify in vivo kinematics for the tibiotalar and subtalar joints. Dynamic tibiotalar and subtalar mean joint angles often exhibited opposing trends during captured stance. During both speeds of walking, the tibiotalar joint had significantly greater dorsi/plantarflexion (D/P) angular ROM than the subtalar joint while the subtalar joint demonstrated greater inversion/eversion (In/Ev) and internal/external rotation (IR/ER) than the tibiotalar joint. During balanced heel-rise, only D/P and In/Ev were significantly different between the tibiotalar and subtalar joints. Translational ROM in the anterior/posterior (AP) direction was significantly greater in the subtalar than the tibiotalar joint during walking at 0.5 m/s. Overall, our results support the long-held belief that the tibiotalar joint is primarily responsible for D/P, while the subtalar joint facilitates In/Ev and IR/ER. However, the subtalar joint provided considerable D/P rotation, and the tibiotalar joint rotated about all three axes, which, along with translational motion, suggests that each joint undergoes complex, 3D motion.